High External Quantum Efficiency Light-Emitting Diodes Enabled by Advanced Heterostructures of Type-II Nanoplatelets

Colloidal quantum wells (CQWs), also known as nanoplatelets (NPLs), are exciting material systems for numerous photonic applications, including lasers and light-emitting diodes (LEDs). Although many successful type-I NPL-LEDs with high device performance have been demonstrated, type-II NPLs are not fully exploited for LED applications, even with alloyed type-II NPLs with enhanced optical properties. Here, we present the development of CdSe/CdTe/CdSe core/crown/crown (multi-crowned) type-II NPLs and systematic investigation of their optical properties, including their comparison with the traditional core/crown counterparts. Unlike traditional type-II NPLs such as CdSe/CdTe, CdTe/CdSe, and CdSe/CdSexTe1–x core/crown heterostructures, here the proposed advanced heterostructure reaps the benefits of having two type-II transition channels, resulting in a high quantum yield (QY) of 83% and a long fluorescence lifetime of 73.3 ns. These type-II transitions were confirmed experimentally by optical measurements and theoretically using electron and hole wave function modeling. Computational study shows that the multi-crowned NPLs provide a better-distributed hole wave function along the CdTe crown, while the electron wave function is delocalized in the CdSe core and CdSe crown layers. As a proof-of-concept demonstration, NPL-LEDs based on these multi-crowned NPLs were designed and fabricated with a record high external quantum efficiency (EQE) of 7.83% among type-II NPL-LEDs. These findings are expected to induce advanced designs of NPL heterostructures to reach a fascinating level of performance, especially in LEDs and lasers.

[1]  J. I. Climente,et al.  Double-crowned 2D semiconductor nanoplatelets with bicolor power-tunable emission , 2022, Nature Communications.

[2]  H. Demir,et al.  High-Performance Deep Red Colloidal Quantum Well Light-Emitting Diodes Enabled by the Understanding of Charge Dynamics. , 2022, ACS nano.

[3]  J. I. Climente,et al.  Highly Charged Excitons and Biexcitons in Type-II Core/Crown Colloidal Nanoplatelets , 2022, The Journal of Physical Chemistry C.

[4]  B. Abécassis,et al.  Curvature and self-assembly of semi-conducting nanoplatelets , 2022, Communications Chemistry.

[5]  W. Sukkabot Atomistic effect of laterally and vertically growth shell on physical behaviours of CdSe/CdTe type-II core/crown and core/shell nanoplatelets: tight-binding theory , 2021, Physica Scripta.

[6]  Hela Boustanji,et al.  Tuning optoelectronic response of lateral core-alloyed crown nanoplatelets: type-II CdSe–CdSe1−x Te x , 2021, Journal of physics. Condensed matter : an Institute of Physics journal.

[7]  D. van Thourhout,et al.  Localization-limited exciton oscillator strength in colloidal CdSe nanoplatelets revealed by the optically induced stark effect , 2021, Light, science & applications.

[8]  Savas Delikanli,et al.  Ultrahigh Green and Red Optical Gain Cross Sections from Solutions of Colloidal Quantum Well Heterostructures. , 2020, The journal of physical chemistry letters.

[9]  J. Qu,et al.  Heterostructures in Two-Dimensional CdSe Nanoplatelets: Synthesis, Optical Properties, and Applications , 2020 .

[10]  A. Riedinger,et al.  Lateral Size Dependence in FRET between Semiconductor Nanoplatelets and Conjugated Fluorophores , 2020 .

[11]  Jiahao Yu,et al.  Optical properties and applications of two‐dimensional CdSe nanoplatelets , 2020 .

[12]  Handong Sun,et al.  Spectrally Wide-Range-Tunable, Efficient, and Bright Colloidal Light-Emitting Diodes of Quasi-2D Nanoplatelets Enabled by Engineered Alloyed Heterostructures , 2020 .

[13]  B. Diroll Colloidal quantum wells for optoelectronic devices , 2020 .

[14]  J. I. Climente,et al.  Emission State Structure and Linewidth Broadening Mechanisms in Type-II CdSe/CdTe Core–Crown Nanoplatelets: A Combined Theoretical–Single Nanocrystal Optical Study , 2020, The Journal of Physical Chemistry C.

[15]  Manoj Sharma,et al.  Two-Dimensional CdSe-Based Nanoplatelets: Their Heterostructures, Doping, Photophysical Properties, and Applications , 2020, Proceedings of the IEEE.

[16]  J. I. Climente,et al.  CdSe/CdS/CdTe Core/Barrier/Crown Nanoplatelets: Synthesis, Optoelectronic Properties, and Multiphoton Fluorescence Upconversion , 2020, ACS nano.

[17]  M. Kovalenko,et al.  Colloidal CdSe Quantum Wells with Graded Shell Composition for Low-Threshold Amplified Spontaneous Emission and Highly Efficient Electroluminescence. , 2019, ACS nano.

[18]  D. Norris,et al.  Compositional Grading for Efficient and Narrowband Emission in CdSe-Based Core/Shell Nanoplatelets , 2019, Chemistry of Materials.

[19]  Handong Sun,et al.  Record High External Quantum Efficiency of 19.2% Achieved in Light‐Emitting Diodes of Colloidal Quantum Wells Enabled by Hot‐Injection Shell Growth , 2019, Advanced materials.

[20]  Savas Delikanli,et al.  Sub-single exciton optical gain threshold in colloidal semiconductor quantum wells with gradient alloy shelling , 2019, Nature Communications.

[21]  Hilmi Volkan Demir,et al.  Orientation-Controlled Nonradiative Energy Transfer to Colloidal Nanoplatelets: Engineering Dipole Orientation Factor. , 2019, Nano letters.

[22]  Dong Choon Hyun,et al.  Heterostructures in two-dimensional colloidal metal chalcogenides: Synthetic fundamentals and applications , 2019, Nano Research.

[23]  R. Schaller,et al.  Reducing the Optical Gain Threshold in Two-Dimensional CdSe Nanoplatelets by the Giant Oscillator Strength Transition Effect. , 2019, The journal of physical chemistry letters.

[24]  Nima Taghipour,et al.  Highly Stable Multicrown Heterostructures of Type-II Nanoplatelets for Ultralow Threshold Optical Gain , 2019, Chemistry of Materials.

[25]  Hilmi Volkan Demir,et al.  Giant Modal Gain Coefficients in Colloidal II-VI Nanoplatelets. , 2018, Nano letters.

[26]  Jian Yuan,et al.  Emergence of Nanoplatelet Light-Emitting Diodes , 2018, Materials.

[27]  Savas Delikanli,et al.  Nanocrystal light-emitting diodes based on type II nanoplatelets , 2018 .

[28]  T. Lian,et al.  A model for optical gain in colloidal nanoplatelets† †Electronic supplementary information (ESI) available: Synthesis procedure, additional transient absorption spectra and kinetics, fitting procedures, and fitting parameters. See DOI: 10.1039/c7sc04294a , 2017, Chemical science.

[29]  Patrick Davidson,et al.  Ligand-induced twisting of nanoplatelets and their self-assembly into chiral ribbons , 2017, Science Advances.

[30]  Hilmi Volkan Demir,et al.  CdSe/CdSe1–xTex Core/Crown Heteronanoplatelets: Tuning the Excitonic Properties without Changing the Thickness , 2017 .

[31]  T. Lian,et al.  Low Threshold Multiexciton Optical Gain in Colloidal CdSe/CdTe Core/Crown Type-II Nanoplatelet Heterostructures. , 2017, ACS nano.

[32]  Hilmi Volkan Demir,et al.  Platelet‐in‐Box Colloidal Quantum Wells: CdSe/CdS@CdS Core/Crown@Shell Heteronanoplatelets , 2016 .

[33]  Savas Delikanli,et al.  Experimental Determination of the Absorption Cross-Section and Molar Extinction Coefficient of Colloidal CdSe Nanoplatelets , 2015 .

[34]  M. Artemyev,et al.  Colloidal synthesis and optical properties of type-II CdSe-CdTe and inverted CdTe-CdSe core-wing heteronanoplatelets. , 2015, Nanoscale.

[35]  Savas Delikanli,et al.  Type-II Colloidal Quantum Wells: CdSe/CdTe Core/Crown Heteronanoplatelets , 2015 .

[36]  T. Lian,et al.  Efficient and ultrafast formation of long-lived charge-transfer exciton state in atomically thin cadmium selenide/cadmium telluride type-II heteronanosheets. , 2015, ACS nano.

[37]  Benoit Dubertret,et al.  Type-II CdSe/CdTe core/crown semiconductor nanoplatelets. , 2014, Journal of the American Chemical Society.

[38]  Vincent Loriette,et al.  Spectroscopy of single CdSe nanoplatelets. , 2012, ACS nano.

[39]  Andrei Schliwa,et al.  Electronic structure and exciton-phonon interaction in two-dimensional colloidal CdSe nanosheets. , 2012, Nano letters.

[40]  B. Dubertret,et al.  Colloidal nanoplatelets with two-dimensional electronic structure. , 2011, Nature materials.

[41]  M. Bawendi,et al.  Type-II quantum dots: CdTe/CdSe(core/shell) and CdSe/ZnTe(core/shell) heterostructures. , 2003, Journal of the American Chemical Society.